苏州大学徐来团队报道了嵌在氮化碳中用于电催化生成多碳产品的四原子簇的设计。相关研究成果发表在2023年3月15日出版的国际知名学术期刊《美国化学会杂志》。

用于电催化CO2和CO还原反应（CORR）的高效稳定催化剂的开发正在积极研究中，但C2产物的选择性差和效率低的问题仍然存在。

研究人员设计了一种二维氮化碳材料（C5N2H2），该材料包含八个N原子，能够配位四个金属原子簇并同时支持C2偶联所需的两个碳氧化物分子。所设计的材料具有优异的导电性和稳定性。在高通量筛选嵌入框架中的多个四金属团簇的催化性能后，研究人员系统地研究了11个候选物的CORR过程。发现，Cu4-C5N2H2对乙烯转化具有优异的选择性和低限制潜力，而Cu2Zn2-C5N2H2对于合成乙醇具有选择性和有效性。

此外，研究人员发现了一种与2D材料柔性相关的新型描述符，以评估生成乙烯的潜在决定步骤。该研究拓宽了少原子CO还原的可能性，并展示了一种新的与底物柔性相关的描述符来预测材料的催化性能。

附：英文原文

Title: Design of a Four-Atom Cluster Embedded in Carbon Nitride for Electrocatalytic Generation of Multi-Carbon Products

Author: Dewei Zhang, Oleg V. Prezhdo, Lai Xu

Issue&Volume: March 15, 2023

Abstract: The development of efficient and stable catalysts for the electrocatalytic CO2 and CO reduction reactions (CORR) is under active investigation, but the problems of poor selectivity and low efficiency for C2 products still exist. We design a two-dimensional carbon nitride material (C5N2H2) that contains an eight N-atom structure capable of coordinating four-metal atom clusters and supporting simultaneously two carbon oxide molecules needed for the C2 coupling. The designed material has excellent electrical conductivity and stability. After high-throughput screening of catalytic performance of multiple four-metal clusters embedded into the framework, we systematically investigate the CORR process of 11 candidates. We find that Cu4-C5N2H2 has superior selectivity and low limiting potential for generating ethylene, while Cu2Zn2-C5N2H2 is selective and efficient to synthesize ethanol. Further, we discover a novel type of descriptor related to 2D material flexibility to evaluate the potential-determining step for generating ethylene. Our report both broadens the possibilities for few-atom CO reduction and demonstrates a novel substrate flexibility-related descriptor to predict the catalytic performance of materials.

DOI: 10.1021/jacs.3c01561

Source: https://pubs.acs.org/doi/10.1021/jacs.3c01561